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Enzymatic reactions in solution drive the convection of confined fluids throughout the enclosing chambers and thereby couple the processes of reaction and convection. In these systems, the energy released from the chemical reactions generates a force, which propels the fluids’ spontaneous motion. Here, we use theoretical and computational modeling to determine how reaction-convection can be harnessed to tailor and control the dynamic behavior of soft matter immersed in solution. Our model system encompasses an array of surface-anchored, flexible posts in a millimeter-sized, fluid-filled chamber. Selected posts are coated with enzymes, which react with dissolved chemicals to produce buoyancy-driven fluid flows. We show that these chemically generated flows exert a force on both the coated (active) and passive posts and thus produce regular, self-organized patterns. Due to the specificity of enzymatic reactions, the posts display controllable kaleidoscopic behavior where one regular pattern is smoothly morphed into another with the addition of certain reactants. These spatiotemporal patterns also form “fingerprints” that distinctly characterize the system, reflecting the type of enzymes used, placement of the enzyme-coated posts, height of the chamber, and bending modulus of the elastic posts. The results reveal how reaction-convection provides concepts for designing soft matter that readily switches among multiple morphologies. This behavior enables microfluidic devices to be spontaneously reconfigured for specific applications without construction of new chambers and the fabrication of standalone sensors that operate without extraneous power sources.
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Programming Fluid Motion Using Multi-Enzyme Micropump Systems
In the presence of appropriate substrates, surface-anchored enzymes can act as pumps and propel fluid through microchambers. Understanding the dynamic interplay between catalytic reactions and fluid flow is vital to enhancing the accuracy and utility of flow technology. Through a combination of experimental observations and numerical modelling, we show that coupled enzyme pumps can exhibit flow enhancement, flow suppression, and changes in the directionality (reversal) of the fluid motion. The pumps’ ability to regulate the flow path is due to the reaction selectivity of the enzymes; the resultant fluid motion is only triggered by the presence of certain reactants. Hence, the reactants and the sequence in which they are present in the solution, and the layout of the enzyme-attached patches form an “instruction set” that guides the flowing solution to specific sites in the system. Such systems can operate as sensors that indicate concentrations of reactants through measurement of the trajectory along which the flow demonstrates maximal speed. The performed simulations suggest that the solutal buoyancy mechanism causes fluid motion and is responsible for all the observed effects. More broadly, our studies provide a new route for forming self-organizing flow systems that can yield fundamental insight into non-equilibrium, dynamical systems.
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- Award ID(s):
- 2234134
- PAR ID:
- 10536480
- Publisher / Repository:
- American Chemical Society
- Date Published:
- Journal Name:
- ACS Applied Materials & Interfaces
- ISSN:
- 1944-8244
- Subject(s) / Keyword(s):
- Enzyme Pumps Buoyancy-Driven Convection Fluid Flow Sensor Catalysis
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acsami.4c07865
